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Transition and main group metals applied to oxidative functionalization of methane and use as high oxygen carriers for rocket propellants

TRANSITION AND MAIN GROUP METALS APPLIED TO OXIDATIVE
FUNCTIONALIZATION OF METHANE AND USE AS HIGH OXYGEN
CARRIERS FOR ROCKET PROPELLANTS
by
CJ Bigler Jones
A Dissertation Presented to the
FACULTY OF THE GRADUATE SCHOOL
UNIVERSITY OF SOUTHERN CALIFORNIA
In Partial Fulfillment of the
Requirements for the Degree
DOCTOR OF PHILOSOPHY
(CHEMISTRY)
August 2007
Copyright 2007 CJ Bigler Jones

This dissertation describes the use of strongly acidic solvents, such as concentrated sulfuric acid, with homogeneous catalysts, such as palladium and gold salts, for the activation and functionalization of methane; and the design, synthesis, and study of ruthenium and osmium complexes in a nitrogen and oxygen ligand environment intended for the low temperature, selective, activation and conversion of methane into oxidatively functionalized products, such as methanol. Also, the principle of using polynitratoaluminate anions, specifically tetranitratoaluminate, as a high oxygen carrier for oxidizer balanced energetic ionic liquids is demonstrated. The structure and properties of other salts of the polynitratoaluminate anions are given. Chapter 2 highlights the use of homogeneous Pd(II) sulfate in concentrated sulfuric acid solution for the direct, selective, oxidative condensation of two methane molecules to acetic acid at 180°C. Chapter 3 focuses on the uses of gold salts for the low temperature conversion of methane to oxidized methyl products, such as methyl bisulfate. Chapter 4 describes the synthesis and characterization of ruthenium and osmium in a nitrogen and oxygen ligand environment. Chapter 5 describes the use of the tetranitratoaluminate anion for oxidizer balanced energetic ionic liquids. Chapter 6 describes the synthesis and characterization of tetramethylammonium and cesium salts of tetranitratoaluminate, pentanitratoaluminate, and hexanitratoaluminate anions.

TRANSITION AND MAIN GROUP METALS APPLIED TO OXIDATIVE
FUNCTIONALIZATION OF METHANE AND USE AS HIGH OXYGEN
CARRIERS FOR ROCKET PROPELLANTS
by
CJ Bigler Jones
A Dissertation Presented to the
FACULTY OF THE GRADUATE SCHOOL
UNIVERSITY OF SOUTHERN CALIFORNIA
In Partial Fulfillment of the
Requirements for the Degree
DOCTOR OF PHILOSOPHY
(CHEMISTRY)
August 2007
Copyright 2007 CJ Bigler Jones